scholarly journals Brown carbon's emission factors and optical characteristics in household biomass burning: developing a novel algorithm for estimating the contribution of brown carbon

2021 ◽  
Vol 21 (4) ◽  
pp. 2329-2341 ◽  
Author(s):  
Jianzhong Sun ◽  
Yuzhe Zhang ◽  
Guorui Zhi ◽  
Regina Hitzenberger ◽  
Wenjing Jin ◽  
...  

Abstract. Recent studies have highlighted the importance of brown carbon (BrC) in various fields, particularly relating to climate change. The incomplete combustion of biomass in open and contained burning conditions is believed to be a significant contributor to primary BrC emissions. So far, few studies have reported the emission factors of BrC from biomass burning, and few studies have specifically addressed which form of light-absorbing carbon, such as black carbon (BC) or BrC, plays a leading role in the total solar light absorption by biomass burning. In this study, the optical integrating sphere (IS) approach was used, with carbon black and humic acid sodium salt as reference materials for BC and BrC, respectively, to distinguish BrC from BC on filter samples. A total of 11 widely used biomass types in China were burned in a typical stove to simulate the real household combustion process. (i) Large differences existed in the emission factors of BrC (EFBrC) among the tested biomass fuels, with a geometric mean EFBrC of 0.71 g kg−1 (0.24–2.09). Both the plant type (herbaceous or ligneous) and burning style (raw or briquetted biomass) might influence the value of EFBrC. The observed reduction in the emissions of light-absorbing carbon (LAC) confirmed an additional benefit of biomass briquetting in climate change mitigation. (ii) The calculated annual BrC emissions from China's household biomass burning amounted to 712 Gg, higher than the contribution from China's household coal combustion (592 Gg). (iii) The average absorption Ångström exponent (AAE) was (2.46±0.53), much higher than that of coal-chunk combustion smoke (AAE=1.30±0.32). (iv) For biomass smoke, the contribution of absorption by BrC to the total absorption by BC+BrC across the strongest solar spectral range of 350–850 nm (FBrC) was 50.8 %. This is nearly twice that for BrC in smoke from household coal combustion (26.5 %). (v) Based on this study, a novel algorithm was developed for estimating the FBrC for perhaps any combustion source (FBrC=0.5519ln⁡AAE+0.0067, R2=0.999); the FBrC value for all global biomass burning (open+contained) (FBrC-entire) was 64.5 % (58.5 %–69.9 %). This corroborates the dominant role of BrC in total biomass burning absorption. Therefore, the inclusion of BrC is not optional but indispensable when considering the climate energy budget, particularly for biomass burning emissions (contained and open).

2020 ◽  
Author(s):  
Jianzhong Sun ◽  
Guorui Zhi ◽  
Regina Hitzenberger ◽  
Yingjun Chen ◽  
Chongguo Tian

Abstract. Recent studies have highlighted the importance of brown carbon (BrC) in various fields, particularly relating to climate change. The incomplete combustion of biomass in open and contained burning conditions is believed to be a significant contributor to primary BrC emissions. So far, few studies have reported the emission factors of BrC from biomass burning, and few studies have specifically addressed which form of light absorbing carbon, such as black carbon (BC) or BrC, plays a leading role in the total solar light absorption of biomass burning. In this study, the optical integrating sphere (IS) approach was used, with carbon black and humic acid sodium salt as reference materials for BC and BrC, respectively, to distinguish BrC from BC on the filter samples. Eleven widely used biomass types in China were burned in a typical stove to simulate the real household combustion process. (i) Large differences existed in the emission factors of BrC (EFBrC) among the tested biomass fuels, with a geomean EFBrC of 0.71 g/kg (0.24, 2.18). Both the plant type (herbaceous or ligneous) and burning style (raw or briquetted biomass) might influence the value of EFBrC. (ii) The calculated annual BrC emissions from China's household biomass burning amounted to 712 Gg, higher than the contribution from China's household coal combustion (592 Gg). (iii) The average absorption Ångström exponent (AAE) was (2.46 ± 0.53), much higher than that of coal-chunks combustion smoke (AAE = 1.30 ± 0.32). (iv) For biomass smoke, the contribution of absorption by BrC to the total absorption by BC + BrC across the strongest solar spectral range of 350–850 nm (FBrC) was 50.8 %. This was nearly twice that for BrC in smoke from household coal combustion (26.5 %). (v) Based on this study, a novel algorithm was developed for estimating the FBrC for any combustion sources (FBrC = 0.5519 lnAAE + 0.0067, R2 = 0.999); the FBrC value for global entire biomass burning (open + contained) (FBrC-entire) was 64.5 % (58.5–69.9 %). This corroborates the dominant role of BrC in total biomass burning absorption. Therefore, BrC is not optional but indispensable when considering the climate energy budget, particularly for biomass burning emissions (contained and open).


2017 ◽  
Author(s):  
Jianzhong Sun ◽  
Guorui Zhi ◽  
Regina Hitzenberger ◽  
Yingjun Chen ◽  
Chongguo Tian ◽  
...  

Abstract. Brown carbon (BrC) draws increasing attention due to its effects on climate and other fields. In China, household coal burned for heating/cooking purposes releases huge amounts of carbonaceous particles every year; however, BrC emissions have rarely been estimated in a persuasive manner due to the unavailable emission characteristics. Here 7 coals jointly covering geological maturity from low to high were burned in 4 typical stoves at both chunk and briquette styles. The optical integrating sphere (IS) method was applied to measure the emission factors (EFs) of BrC and BC via an iterative process using the different spectral dependence of light absorption for BrC and BC. It is found that (i) the average EFs of BrC for anthracite coal chunks and briquettes are (1.08 ± 0.80) g kg−1 and (1.52 ± 0.16) g kg−1, respectively, and those for bituminous coal chunks and briquettes are (8.59 ± 2.70) g kg−1 and (4.01 ± 2.19) g kg−1, respectively, reflecting a more significant decline of BrC EFs for bituminous coals than for anthracites due to briquetting, (ii) the BrC EF peaks at the middle of coal's geological maturity, displaying a bell shaped curve between EF and volatile matter (Vdaf), (iii) the calculated BrC emissions from China's residential coal burning amounted to 592 Gg (1 Gg = 109 g) in 2013, which is nearly half of China's total BC emissions, (iv) absorption Ångström exponent (AAEs) of all coal briquettes are higher than those of coal chunks, indicating that the measure of coal briquetting increases the BrC / BC emission ratio and thus offsets some of the climate cooling effect of briquetting, and (v) in the scenario of current household coal burning in China, solar light absorption by BrC (350–850 nm in this study) accounts for more than a quarter (0.265) of the total absorption. This implies the significance of BrC to climate modeling.


2016 ◽  
Vol 16 (15) ◽  
pp. 9549-9561 ◽  
Author(s):  
Rudra P. Pokhrel ◽  
Nick L. Wagner ◽  
Justin M. Langridge ◽  
Daniel A. Lack ◽  
Thilina Jayarathne ◽  
...  

Abstract. Single-scattering albedo (SSA) and absorption Ångström exponent (AAE) are two critical parameters in determining the impact of absorbing aerosol on the Earth's radiative balance. Aerosol emitted by biomass burning represent a significant fraction of absorbing aerosol globally, but it remains difficult to accurately predict SSA and AAE for biomass burning aerosol. Black carbon (BC), brown carbon (BrC), and non-absorbing coatings all make substantial contributions to the absorption coefficient of biomass burning aerosol. SSA and AAE cannot be directly predicted based on fuel type because they depend strongly on burn conditions. It has been suggested that SSA can be effectively parameterized via the modified combustion efficiency (MCE) of a biomass burning event and that this would be useful because emission factors for CO and CO2, from which MCE can be calculated, are available for a large number of fuels. Here we demonstrate, with data from the FLAME-4 experiment, that for a wide variety of globally relevant biomass fuels, over a range of combustion conditions, parameterizations of SSA and AAE based on the elemental carbon (EC) to organic carbon (OC) mass ratio are quantitatively superior to parameterizations based on MCE. We show that the EC ∕ OC ratio and the ratio of EC ∕ (EC + OC) both have significantly better correlations with SSA than MCE. Furthermore, the relationship of EC ∕ (EC + OC) with SSA is linear. These improved parameterizations are significant because, similar to MCE, emission factors for EC (or black carbon) and OC are available for a wide range of biomass fuels. Fitting SSA with MCE yields correlation coefficients (Pearson's r) of  ∼  0.65 at the visible wavelengths of 405, 532, and 660 nm while fitting SSA with EC / OC or EC / (EC + OC) yields a Pearson's r of 0.94–0.97 at these same wavelengths. The strong correlation coefficient at 405 nm (r =  0.97) suggests that parameterizations based on EC / OC or EC / (EC + OC) have good predictive capabilities even for fuels in which brown carbon absorption is significant. Notably, these parameterizations are effective for emissions from Indonesian peat, which have very little black carbon but significant brown carbon (SSA  =  0.990 ± 0.001 at 532 and 660 nm, SSA  =  0.937 ± 0.011 at 405 nm). Finally, we demonstrate that our parameterization based on EC / (EC + OC) accurately predicts SSA during the first few hours of plume aging with data from Yokelson et al. (2009) gathered during a biomass burning event in the Yucatán Peninsula of Mexico.


2020 ◽  
Author(s):  
Ting Wang ◽  
Rujin Huang ◽  
Lu Yang ◽  
Wei Yuan ◽  
Yuquan Gong

<p>Atmospheric brown carbon (BrC) has significant impact on Earth’s radiative budget. However, due to our very limited knowledge about the relationship between BrC light absorption and the associated sources, the estimation for radiative effects of BrC is still largely constrained. In this study, we combine ultraviolet−visible (UV−vis) spectroscopy measurements and chemical analyses of BrC samples collected from January to December 2015 in urban Beijing, to investigated the sources of atmospheric BrC. The multiple liner regression model was applied to apportion the contributions of individual primary and secondary organic aerosol (OA) source components to light absorption of BrC. Our results indicated that biomass burning emission and secondary formation are highly absorbing up to 500 nm, and their contributions increased with the wavelengths. In contrast, the contribution of traffic emission and coal combustion to total absorption decreased with the wavelength and the large contributions were mostly found at shorter wavelengths. Then the mass absorption efficiency (MAE) of major light-absorbing components were estimated, which can provide a support to estimate the impact of BrC from these sources on the climate. The positive matrix factorization model were also used to verify the contributions of different source components of BrC absorption at 365 nm. The results consistently demonstrate that the biomass burning and secondary formation contributes significantly to the overall absorption, followed by coal combustion and traffic emission.</p>


2017 ◽  
Vol 17 (7) ◽  
pp. 4769-4780 ◽  
Author(s):  
Jianzhong Sun ◽  
Guorui Zhi ◽  
Regina Hitzenberger ◽  
Yingjun Chen ◽  
Chongguo Tian ◽  
...  

Abstract. Brown carbon (BrC) draws increasing attention due to its effects on climate and other environmental factors. In China, household coal burned for heating and cooking purposes releases huge amounts of carbonaceous particles every year; however, BrC emissions have rarely been estimated in a persuasive manner due to the unavailable emission characteristics. Here, seven coals jointly covering geological maturity from low to high were burned in four typical stoves as both chunk and briquette styles. The optical integrating sphere (IS) method was applied to measure the emission factors (EFs) of BrC and black carbon (BC) via an iterative process using the different spectral dependence of light absorption for BrC and BC and using humic acid sodium salt (HASS) and carbon black (CarB) as reference materials. The following results have been found: (i) the average EFs of BrC for anthracite coal chunks and briquettes are 1.08 ± 0.80 and 1.52 ± 0.16 g kg−1, respectively, and those for bituminous coal chunks and briquettes are 8.59 ± 2.70 and 4.01 ± 2.19 g kg−1, respectively, reflecting a more significant decline in BrC EFs for bituminous coals than for anthracites due to briquetting. (ii) The BrC EF peaks at the middle of coal's geological maturity, displaying a bell-shaped curve between EF and volatile matter (Vdaf). (iii) The calculated BrC emissions from China's residential coal burning amounted to 592 Gg (1 Gg  =  109 g) in 2013, which is nearly half of China's total BC emissions. (iv) The absorption Ångström exponents (AAEs) of all coal briquettes are higher than those of coal chunks, indicating that the measure of coal briquetting increases the BrC ∕ BC emission ratio and thus offsets some of the climate cooling effect of briquetting. (v) In the scenario of current household coal burning in China, solar light absorption by BrC (350–850 nm in this study) accounts for more than a quarter (0.265) of the total absorption. This implies the significance of BrC to climate modeling.


2016 ◽  
Author(s):  
Rudra P. Pokhrel ◽  
Nick L. Wagner ◽  
Justin M. Langridge ◽  
Daniel A. Lack ◽  
Thilina Jayarathne ◽  
...  

Abstract. Single scattering albedo (SSA) and absorption angstrom exponent (AAE) are two critical parameters in determining the impact of absorbing aerosol on the Earth's radiative balance. Aerosol emitted by biomass burning represent a significant fraction of absorbing aerosol globally, but it remains difficult to accurately predict SSA and AAE for biomass burning aerosol. Black carbon (BC), brown carbon (BrC), and non-absorbing coatings all make significant contributions to the absorption coefficient of biomass burning aerosol. SSA and AAE cannot be directly inferred based on fuel type because they depend strongly on burn conditions. It has been suggested that SSA can be effectively parameterized via the modified combustion efficiency (MCE) of a biomass-burning event and that this would be useful because emission factors for the MCE of a large number of fuels are available. Here we demonstrate, with data from the FLAME-4 experiment, that for a wide variety of globally relevant biomass fuels, over a range of combustion conditions, parameterizations of SSA and AAE based on the elemental carbon (EC) to organic carbon (OC) mass ratio are quantitatively superior to parameterizations based on MCE. We show that the EC/OC ratio and the ratio of EC/(EC + OC) both have significantly better correlations with SSA than MCE. Furthermore, the relationship of EC/(EC + OC) with SSA is linear. These improved parameterizations are significant because, similar to MCE, emission factors for EC (or black carbon) and OC are available for a wide range of biomass fuels. Fitting SSA with MCE yields correlation coefficients (Pearson's r) of ~ 0.65 at the visible wavelengths of 405, 532, and 660 nm while fitting SSA with EC/OC or EC/(EC + OC) yields a Pearson's r of 0.94–0.97 at these same wavelengths. The strong correlation coefficient at 405 nm (r = 0.97) suggests that parameterizations based on EC/OC or EC/(EC + OC) have good predictive capabilities even for fuels in which brown carbon absorption is significant. Notably, these parameterizations are effective for emissions from Indonesian peat, which have very little black carbon but significant brown carbon (SSA = 0.99 ± 0.07 at 532 and 660 nm, SSA = 0.93 ± 0.06 at 405 nm). Finally, we demonstrate that our parameterization based on EC/(EC + OC) accurately predicts SSA during the first few hours of plume aging with data from Yokelson et al. (2009) gathered during a biomass burning event in the Yucatan Peninsula of Mexico.


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